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Browsing by Author "Liu, Shengwen"
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Item Atomically dispersed iron sites with a nitrogen–carbon coating as highly active and durable oxygen reduction catalysts for fuel cells(Springer Nature, 2022) Liu, Shengwen; Li, Chenzhao; Zachman, Michael J.; Zeng, Yachao; Yu, Haoran; Li, Boyang; Wang, Maoyu; Braaten, Jonathan; Liu, Jiawei; Meyer, Harry M., III; Lucero, Marcos; Kropf, A. Jeremy; Alp, Esen E.; Gong, Qing; Shi, Qiurong; Feng, Zhenxing; Xu, Hui; Wang, Guofeng; Myers, Deborah J.; Xie, Jian; Cullen, David A.; Litster, Shawn; Wu, Gang; Mechanical and Energy Engineering, Purdue School of Engineering and TechnologyNitrogen-coordinated single atom iron sites (FeN4) embedded in carbon (Fe–N–C) are the most active platinum group metal-free oxygen reduction catalysts for proton-exchange membrane fuel cells. However, current Fe–N–C catalysts lack sufficient long-term durability and are not yet viable for practical applications. Here we report a highly durable and active Fe–N–C catalyst synthesized using heat treatment with ammonia chloride followed by high-temperature deposition of a thin layer of nitrogen-doped carbon on the catalyst surface. We propose that catalyst stability is improved by converting defect-rich pyrrolic N-coordinated FeN4 sites into highly stable pyridinic N-coordinated FeN4 sites. The stability enhancement is demonstrated in membrane electrode assemblies using accelerated stress testing and a long-term steady-state test (>300 h at 0.67 V), approaching a typical Pt/C cathode (0.1 mgPt cm−2). The encouraging stability improvement represents a critical step in developing viable Fe–N–C catalysts to overcome the cost barriers of hydrogen fuel cells for numerous applications.Item Effects of Ink Formulation on the Structure and Performance of PGM-Free Catalyst Layer in PEMFCs(IOP, 2021) Li, Chenzhao; Liu, Shengwen; Zeng, Yachao; Liu, Yadong; Wu, Gang; Cullen, David A.; Xie, Jian; Mechanical and Energy Engineering, Purdue School of Engineering and TechnologyPlatinum group metal (PGM) catalysts are the major electrocatalysts for oxygen reduction reaction (ORR) in the polymer electrolyte membrane fuel cells (PEMFCs). The cost becomes unaffordable if the PEMFC is in massive application. The PGM-Free catalyst shows very promising activity in rotation disk electrode (RDE) testing. The half-wave potential could reach 0.91 V versus standard hydrogen electrode (SHE). However, in a membrane electrode assembly (MEA), the performance of PGM-Free catalysts is not good enough to replace the PGM catalysts. Since the PGM-free catalysts are so different from the PGM catalysts in terms of catalytic activity, stability, surface conditions, particle size, etc., the fabrication of PGM-Free catalyst MEA cannot simply copy the method of making PGM MEA. We proposed a novel method of fabricating PGM-Free catalyst MEA, so that the intrinsic catalyst activity from RDE can be translated into MEA performance. The method is based on the catalyst coated membrane (CCM) method using optimized ionomer to carbon (I/C) ratio and solvent mixture of catalyst ink. Using this method, the PGM-free catalyst MEA achieved the current density 44.9 mA cm-2 at 0.9 V iR-free in H2/O2 and 150 mA cm-2 at 0.8 V in H2/air, which surpassed the performance targets of US Department of Energy (DOE)for PGM-Free catalyst MEA. The property (solvent composition, dispersion of catalyst and ionomer in an ink), structure (pore structure) and the MEA performance have been characterized using, mercury intrusion porosimetry (MIP), MEA testing. A property-structure-performance relationship has been established.Item Regulated Viral BDNF Delivery in Combination with Schwann Cells Promotes Axonal Regeneration through Capillary Alginate Hydrogels after Spinal Cord Injury(Elsevier, 2017-09) Liu, Shengwen; Sandner, Beatrice; Schackel, Thomas; Nicholson, LaShae; Chtarto, Abdelwahed; Tenenbaum, Liliane; Puttagunta, Radhika; Müller, Rainer; Weidner, Norbert; Blesch, Armin; Department of Neurological Surgery, School of MedicineGrafting of cell-seeded alginate capillary hydrogels into a spinal cord lesion site provides an axonal bridge while physically directing regenerating axonal growth in a linear pattern. However, without an additional growth stimulus, bridging axons fail to extend into the distal host spinal cord. Here we examined whether a combinatory strategy would support regeneration of descending axons across a cervical (C5) lateral hemisection lesion in the rat spinal cord. Following spinal cord transections, Schwann cell (SC)-seeded alginate hydrogels were grafted to the lesion site and AAV5 expressing brain-derived neurotrophic factor (BDNF) under control of a tetracycline-regulated promoter was injected caudally. In addition, we examined whether SC injection into the caudal spinal parenchyma would further enhance regeneration of descending axons to re-enter the host spinal cord. Our data show that both serotonergic and descending axons traced by biotinylated dextran amine (BDA) extend throughout the scaffolds. The number of regenerating axons is significantly increased when caudal BDNF expression is activated and transient BDNF delivery is able to sustain axons after gene expression is switched off. Descending axons are confined to the caudal graft/host interface even with continuous BDNF expression for 8 weeks. Only with a caudal injection of SCs, a pathway facilitating axonal regeneration through the host/graft interface is generated allowing axons to successfully re-enter the caudal spinal cord.Item Targeted tissue engineering: hydrogels with linear capillary channels for axonal regeneration after spinal cord injury(Medknow Publications, 2018-04) Liu, Shengwen; Blesch, Armin; Neurological Surgery, School of MedicineSpinal cord injury (SCI) frequently results in the permanent loss of function below the level of injury due to the failure of axonal regeneration in the adult mammalian central nervous system (CNS). The limited intrinsic growth capacity of adult neurons, a lack of growth-promoting factors and the multifactorial inhibitory microenvironment around the lesion site contribute to the lack of axonal regeneration. Strategies such as transplantation of cells, delivery of bioactive compounds and gene transfer have been investigated as a means to promote axonal regrowth through the lesion, to form new synaptic connections and to improve functional outcomes. Although growth of some axonal populations can be robustly enhanced by cellular implants alone or in combination with neurotrophic factors, axons usually extend in random orientation and even reverse growth direction in the lesion site (Figure 1A) (Gros et al., 2010; Günther et al., 2015). Thus, regenerating axons often fail to approach the distal edge of the lesion site, a pre-requisite for proper contact with spared host neurons. The lack of a 3-dimensional organization in the injury site is therefore an additional barrier for successful axonal bridging. Two approaches, physical guidance through structured scaffolds and chemical guidance by growth factor gradients, have emerged as potential means to provide directional cues for axonal growth through the lesion.